Semiconductor-based photoelectrochemical (PEC) test protocols offer a viable solution for developing efficient individual health monitoring by converting light and chemical energy into electrical signals. However, slow reaction kinetics and electron–hole complexation at the interface limit their practical application. Here, we reported a triple-engineered CdS nanohierarchical structures (CdS NHs) modification scheme including morphology, defective states, and heterogeneous structure to achieve precise monitoring of the neurotransmitter dopamine (DA) in plasma and noninvasive body fluids. By precisely manipulating the Cd–S precursor, we achieved precise control over ternary CdS NHs and obtained well-defined layered self-assembled CdS NHs through a surface carbon treatment. The integration of defect states and the thin carbon layer effectively established carrier directional transfer pathways, thereby enhancing interface reaction sites and improving the conversion efficiency. The CdS NHs microelectrode fabricated demonstrated a remarkable negative response toward DA, thereby enabling the development of a miniature self-powered PEC device for precise quantification in human saliva. Additionally, the utilization of density functional theory calculations elucidated the structural characteristics of DA and the defect state of CdS, thus establishing crucial theoretical groundwork for optimizing the polymerization process of DA. The present study offers a potential engineering approach for developing high energy conversion efficiency PEC semiconductors as well as proposing a novel concept for designing sensitive testing strategies.

中文翻译：

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塑造神经递质传感器的未来：为最先进的自供电光电化学设备定制 CdS 纳米结构


基于半导体的光电化学 (PEC) 测试协议通过将光和化学能转换为电信号，为开发高效的个人健康监测提供了可行的解决方案。然而，缓慢的反应动力学和界面处的电子-空穴络合限制了它们的实际应用。在这里，我们报道了一种三重设计的CdS纳米分级结构（CdS NHs）修饰方案，包括形态、缺陷状态和异质结构，以实现血浆和非侵入性体液中神经递质多巴胺（DA）的精确监测。通过精确操控Cd-S前驱体，我们实现了对三元CdS NH的精确控制，并通过表面碳处理获得了清晰的层状自组装CdS NH。缺陷态和薄碳层的整合有效地建立了载流子定向转移路径，从而增强了界面反应位点并提高了转换效率。制造的 CdS NHs 微电极表现出对 DA 的显着负响应，从而能够开发微型自供电 PEC 装置，用于人类唾液的精确定量。此外，利用密度泛函理论计算阐明了DA的结构特征和CdS的缺陷态，从而为优化DA的聚合过程奠定了重要的理论基础。本研究为开发高能量转换效率PEC半导体提供了一种潜在的工程方法，并提出了设计敏感测试策略的新概念。